Tailoring Electrode Microstructure via Ink Content to Enable Improved Rated Power Performance for Platinum Cobalt/High Surface Area Carbon Based Polymer Electrolyte Fuel Cells

Van Cleve, Timothy; Wang, Guanxiong; Mooney, Mason; Cetinbas, C. Firat; Kariuki, Nancy; Park, Jaehyung; Farghaly, Ahmed; Myers, Deborah; Neyerlin, Kenneth C.

doi:10.1016/j.jpowsour.2020.228889

Tailoring Electrode Microstructure via Ink Content to Enable Improved Rated Power Performance for Platinum Cobalt/High Surface Area Carbon Based Polymer Electrolyte Fuel Cells

Journal Article · Mon Sep 21 04:00:00 EDT 2020 · Journal of Power Sources

DOI:https://doi.org/10.1016/j.jpowsour.2020.228889· OSTI ID:1677442

Van Cleve, Timothy; Wang, Guanxiong; Mooney, Mason; Cetinbas, C. Firat; Kariuki, Nancy; Park, Jaehyung; Farghaly, Ahmed; Myers, Deborah; Neyerlin, Kenneth C.

Improvements in polymer electrolyte fuel cell (PEFC) electrode performance have primarily focused on catalyst and ionomer developments, marginalizing the importance of catalyst ink formulation. Herein, the effect of ink formulation is examined across a series of cathodes comprised of PtCo supported on high surface area carbon (PtCo/HSC) and Nafion ionomer using an array of in situ electrochemical and ex situ characterization techniques. In contrast to prior work on Pt/Vu systems, ink water content had little effect on the electrochemically determined ionomer coverage for the PtCo/HSC electrocatalyst examined here. Characterization using nano-scale resolution X-ray computed tomography (nano-CT) demonstrated that water-rich ink formulations lead to a reduction in aggregate size (ionomer + PtCo/HSC), improving local O2 transport. This understanding, combined with the use of a commercially-available electrocatalyst was used to produced state-of-the-art membrane electrode assemblies with Pt loadings of 0.03/0.08 mgPt/cm2 on the anode and cathode respectively, having; i) > 1 A/mgPt (0.9 ViR-free, 150 kPa, 80 °C, 100% RH, H2/O2), ii) 320 mA/cm2 at 0.8 V, 150 kPa, 80 °C, 100% RH, H2/Air), and iii) > 1 W/cm2elec at rated power (0.67 V, 250 kPa, 94 °C, 65% RH, H2/Air) or < 0.11 gPt/kWrated.

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Hydrogen and Fuel Cell Technologies Office (EE-3F)

DOE Contract Number:: AC36-08GO28308

OSTI ID:: 1677442

Report Number(s):: NREL/JA-5900-76984; MainId:24947; UUID:bb5ac9cc-8289-4566-b1ff-97e65f93b019; MainAdminID:18631

Journal Information:: Journal of Power Sources, Journal Name: Journal of Power Sources Vol. 482

Country of Publication:: United States

Language:: English

References (65)

Fe Stabilization by Intermetallic L1 ₀ -FePt and Pt Catalysis Enhancement in L1 ₀ -FePt/Pt Nanoparticles for Efficient Oxygen Reduction Reaction in Fuel Cells Li, Junrui; Xi, Zheng; Pan, Yung-Tin Journal of the American Chemical Society, Vol. 140, Issue 8 https://doi.org/10.1021/jacs.7b12829	journal	February 2018
Analysis of the Microstructure Formation Process and Its Influence on the Performance of Polymer Electrolyte Fuel-Cell Catalyst Layers Takahashi, Shinichi; Mashio, Tetsuya; Horibe, Norifumi ChemElectroChem, Vol. 2, Issue 10 https://doi.org/10.1002/celc.201500131	journal	July 2015
Microstructural Analysis and Transport Resistances of Low-Platinum-Loaded PEFC Electrodes Cetinbas, Firat C.; Wang, Xiaohua; Ahluwalia, Rajesh K. Journal of The Electrochemical Society, Vol. 164, Issue 14 https://doi.org/10.1149/2.1111714jes	journal	January 2017
Impact of Compressive Stress on MEA Pore Structure and Its Consequence on PEMFC Performance Sassin, M. B.; Garsany, Y.; Gould, B. D. Journal of The Electrochemical Society, Vol. 163, Issue 8 https://doi.org/10.1149/2.0291608jes	journal	January 2016
Effects of Porous Carbon Morphology, Agglomerate Structure and Relative Humidity on Local Oxygen Transport Resistance Cetinbas, Firat C.; Ahluwalia, Rajesh K.; Kariuki, Nancy N. Journal of The Electrochemical Society, Vol. 167, Issue 1 https://doi.org/10.1149/2.0082001JES	journal	September 2019
Determination of O ₂ Mass Transport at the Pt \| PFSA Ionomer Interface under Reduced Relative Humidity Novitski, David; Holdcroft, Steven ACS Applied Materials & Interfaces, Vol. 7, Issue 49 https://doi.org/10.1021/acsami.5b08720	journal	December 2015
Measurement of Oxygen Transport Resistance in PEM Fuel Cells by Limiting Current Methods Baker, Daniel R.; Caulk, David A.; Neyerlin, Kenneth C. Journal of The Electrochemical Society, Vol. 156, Issue 9 https://doi.org/10.1149/1.3152226	journal	January 2009
Integration of TomoPy and the ASTRA toolbox for advanced processing and reconstruction of tomographic synchrotron data Pelt, Daniël M.; Gürsoy, Dogˇa; Palenstijn, Willem Jan Journal of Synchrotron Radiation, Vol. 23, Issue 3 https://doi.org/10.1107/S1600577516005658	journal	April 2016
Tailoring the Membrane-Electrode Interface in PEM Fuel Cells: A Review and Perspective on Novel Engineering Approaches Breitwieser, Matthias; Klingele, Matthias; Vierrath, Severin Advanced Energy Materials, Vol. 8, Issue 4 https://doi.org/10.1002/aenm.201701257	journal	September 2017
A Review of the Terms Agglomerate and Aggregate with a Recommendation for Nomenclature Used in Powder and Particle Characterization Nichols, Gary; Byard, Stephen; Bloxham, Mark J. Journal of Pharmaceutical Sciences, Vol. 91, Issue 10 https://doi.org/10.1002/jps.10191	journal	October 2002
Analysis of Oxygen-Transport Diffusion Resistance in Proton-Exchange-Membrane Fuel Cells Nonoyama, Nobuaki; Okazaki, Shinobu; Weber, Adam Z. Journal of The Electrochemical Society, Vol. 158, Issue 4 https://doi.org/10.1149/1.3546038	journal	January 2011
Impact of Substrate and Processing on Confinement of Nafion Thin Films Kusoglu, Ahmet; Kushner, Douglas; Paul, Devproshad K. Advanced Functional Materials, Vol. 24, Issue 30 https://doi.org/10.1002/adfm.201304311	journal	April 2014
Control of Architecture in Rhombic Dodecahedral Pt–Ni Nanoframe Electrocatalysts Becknell, Nigel; Son, Yoonkook; Kim, Dohyung Journal of the American Chemical Society, Vol. 139, Issue 34 https://doi.org/10.1021/jacs.7b05584	journal	August 2017
Nanoscale 3D imaging at the Advanced Photon Source De Andrade, Vincent; Deriy, Alex; Wojcik, Michael J. SPIE Newsroom https://doi.org/10.1117/2.1201604.006461	journal	May 2016
Electrical resistance and microstructure of typical gas diffusion layers for proton exchange membrane fuel cell under compression Qiu, Diankai; Janßen, Holger; Peng, Linfa Applied Energy, Vol. 231 https://doi.org/10.1016/j.apenergy.2018.09.117	journal	December 2018
Support materials for PEMFC and DMFC electrocatalysts—A review Sharma, Surbhi; Pollet, Bruno G. Journal of Power Sources, Vol. 208 https://doi.org/10.1016/j.jpowsour.2012.02.011	journal	June 2012
Characterizing Electrolyte and Platinum Interface in PEM Fuel Cells Using CO Displacement Garrick, Taylor R.; Moylan, Thomas E.; Yarlagadda, Venkata Journal of The Electrochemical Society, Vol. 164, Issue 2 https://doi.org/10.1149/2.0551702jes	journal	December 2016
Ultra-small-angle X-ray scattering at the Advanced Photon Source Ilavsky, Jan; Jemian, Pete R.; Allen, Andrew J. Journal of Applied Crystallography, Vol. 42, Issue 3 https://doi.org/10.1107/S0021889809008802	journal	April 2009
Exceptional Oxygen Reduction Reaction Activity and Durability of Platinum–Nickel Nanowires through Synthesis and Post-Treatment Optimization Alia, Shaun M.; Ngo, Chilan; Shulda, Sarah ACS Omega, Vol. 2, Issue 4 https://doi.org/10.1021/acsomega.7b00054	journal	April 2017
Water Management in Cathode Catalyst Layers of PEM Fuel Cells Eikerling, M. Journal of The Electrochemical Society, Vol. 153, Issue 3 https://doi.org/10.1149/1.2160435	journal	January 2006
The Priority and Challenge of High-Power Performance of Low-Platinum Proton-Exchange Membrane Fuel Cells Kongkanand, Anusorn; Mathias, Mark F. The Journal of Physical Chemistry Letters, Vol. 7, Issue 7 https://doi.org/10.1021/acs.jpclett.6b00216	journal	March 2016
Oxidation of Platinum Nickel Nanowires to Improve Durability of Oxygen-Reducing Electrocatalysts Alia, Shaun M.; Pylypenko, Svitlana; Dameron, Arrelaine Journal of The Electrochemical Society, Vol. 163, Issue 3 https://doi.org/10.1149/2.0081605jes	journal	January 2016
Impact of Platinum Loading and Catalyst Layer Structure on PEMFC Performance Owejan, Jon P.; Owejan, Jeanette E.; Gu, Wenbin Journal of The Electrochemical Society, Vol. 160, Issue 8 https://doi.org/10.1149/2.072308jes	journal	January 2013
Fabrication Method for Laboratory-Scale High-Performance Membrane Electrode Assemblies for Fuel Cells Sassin, Megan B.; Garsany, Yannick; Gould, Benjamin D. Analytical Chemistry, Vol. 89, Issue 1 https://doi.org/10.1021/acs.analchem.6b03005	journal	December 2016
Measurement of Catalyst Layer Electrolyte Resistance in PEFCs Using Electrochemical Impedance Spectroscopy Makharia, Rohit; Mathias, Mark F.; Baker, Daniel R. Journal of The Electrochemical Society, Vol. 152, Issue 5 https://doi.org/10.1149/1.1888367	journal	January 2005
High power, Low-Pt membrane electrode assemblies for proton exchange membrane fuel cells Garsany, Yannick; Atkinson, Robert W.; Gould, Benjamin D. Journal of Power Sources, Vol. 408 https://doi.org/10.1016/j.jpowsour.2018.10.073	journal	December 2018
Rheological Investigation on the Microstructure of Fuel Cell Catalyst Inks Khandavalli, Sunilkumar; Park, Jae Hyung; Kariuki, Nancy N. ACS Applied Materials & Interfaces, Vol. 10, Issue 50 https://doi.org/10.1021/acsami.8b15039	journal	December 2018
Effect of gas diffusion layer compression on PEM fuel cell performance Ge, Jiabin; Higier, Andrew; Liu, Hongtan Journal of Power Sources, Vol. 159, Issue 2 https://doi.org/10.1016/j.jpowsour.2005.11.069	journal	September 2006
New results of PEFC electrodes produced by the DLR dry preparation technique Gülzow, Erich; Kaz, Till Journal of Power Sources, Vol. 106, Issue 1-2 https://doi.org/10.1016/S0378-7753(01)01030-8	journal	April 2002
Modeling Air Electrodes with Low Platinum Loading Darling, Robert Journal of The Electrochemical Society, Vol. 166, Issue 7 https://doi.org/10.1149/2.0101907jes	journal	January 2019
Agglomerates in Polymer Electrolyte Fuel Cell Electrodes: Part II. Transport Characterization Cetinbas, Firat C.; Ahluwalia, Rajesh K. Journal of The Electrochemical Society, Vol. 165, Issue 13 https://doi.org/10.1149/2.0301813jes	journal	January 2018
Inherent Acidity of Perfluorosulfonic Acid Ionomer Dispersions and Implications for Ink Aggregation Berlinger, Sarah A.; McCloskey, Bryan D.; Weber, Adam Z. The Journal of Physical Chemistry B, Vol. 122, Issue 31 https://doi.org/10.1021/acs.jpcb.8b06493	journal	July 2018
Boosting Fuel Cell Performance with Accessible Carbon Mesopores Yarlagadda, Venkata; Carpenter, Michael K.; Moylan, Thomas E. ACS Energy Letters, Vol. 3, Issue 3 https://doi.org/10.1021/acsenergylett.8b00186	journal	February 2018
Dictating Pt-Based Electrocatalyst Performance in Polymer Electrolyte Fuel Cells, from Formulation to Application Van Cleve, Tim; Khandavalli, Sunilkumar; Chowdhury, Anamika ACS Applied Materials & Interfaces, Vol. 11, Issue 50 https://doi.org/10.1021/acsami.9b17614	journal	November 2019
Utilizing ink composition to tune bulk-electrode gas transport, performance, and operational robustness for a Fe–N–C catalyst in polymer electrolyte fuel cell Osmieri, Luigi; Wang, Guanxiong; Cetinbas, Firat C. Nano Energy, Vol. 75 https://doi.org/10.1016/j.nanoen.2020.104943	journal	September 2020
Irena : tool suite for modeling and analysis of small-angle scattering Ilavsky, Jan; Jemian, Peter R. Journal of Applied Crystallography, Vol. 42, Issue 2 https://doi.org/10.1107/S0021889809002222	journal	February 2009
Understanding inks for porous-electrode formation Hatzell, Kelsey B.; Dixit, Marm B.; Berlinger, Sarah A. J. Mater. Chem. A, Vol. 5, Issue 39 https://doi.org/10.1039/C7TA07255D	journal	January 2017
Ink Solvent Dependence of the Ionomer Distribution in the Catalyst Layer of a PEMFC Orfanidi, Alin; Rheinländer, Philipp J.; Schulte, Nicole Journal of The Electrochemical Society, Vol. 165, Issue 14 https://doi.org/10.1149/2.1251814jes	journal	January 2018
The Impact of Platinum Loading on Oxygen Transport Resistance Greszler, Thomas A.; Caulk, David; Sinha, Puneet Journal of The Electrochemical Society, Vol. 159, Issue 12 https://doi.org/10.1149/2.061212jes	journal	January 2012
Performance of advanced automotive fuel cell systems with heat rejection constraint Ahluwalia, R. K.; Wang, X.; Steinbach, A. J. Journal of Power Sources, Vol. 309 https://doi.org/10.1016/j.jpowsour.2016.01.060	journal	March 2016
Influence of the Gas Diffusion Layer Compression on the Oxygen Transport in PEM Fuel Cells at High Water Saturation Levels Simon, Christoph; Hasché, Frédéric; Gasteiger, Hubert A. Journal of The Electrochemical Society, Vol. 164, Issue 6 https://doi.org/10.1149/2.0691706jes	journal	January 2017
Pt alloy oxygen-reduction electrocatalysts: Synthesis, structure, and property Wang, Xiao Xia; Sokolowski, Joshua; Liu, Hui Chinese Journal of Catalysis, Vol. 41, Issue 5 https://doi.org/10.1016/S1872-2067(19)63407-8	journal	May 2020
Effects of carbon supports on Pt distribution, ionomer coverage and cathode performance for polymer electrolyte fuel cells Park, Young-Chul; Tokiwa, Haruki; Kakinuma, Katsuyoshi Journal of Power Sources, Vol. 315 https://doi.org/10.1016/j.jpowsour.2016.02.091	journal	May 2016
Multimetallic Core/Interlayer/Shell Nanostructures as Advanced Electrocatalysts Kang, Yijin; Snyder, Joshua; Chi, Miaofang Nano Letters, Vol. 14, Issue 11 https://doi.org/10.1021/nl5028205	journal	October 2014
Characterization of 9Cr-1MoVNb steel by anomalous small-angle X-ray scattering Jemian, P. R.; Weertman, J. R.; Long, G. G. Acta Metallurgica et Materialia, Vol. 39, Issue 11 https://doi.org/10.1016/0956-7151(91)90062-6	journal	November 1991
The impact of short side chain ionomer on polymer electrolyte membrane fuel cell performance and durability Shahgaldi, Samaneh; Alaefour, Ibrahim; Li, Xianguo Applied Energy, Vol. 217 https://doi.org/10.1016/j.apenergy.2018.02.154	journal	May 2018
Resolving Electrode Morphology’s Impact on Platinum Group Metal-Free Cathode Performance Using Nano-CT of 3D Hierarchical Pore and Ionomer Distribution Komini Babu, Siddharth; Chung, Hoon T.; Zelenay, Piotr ACS Applied Materials & Interfaces, Vol. 8, Issue 48 https://doi.org/10.1021/acsami.6b08844	journal	November 2016
Nanofiber Electrodes with Low Platinum Loading for High Power Hydrogen/Air PEM Fuel Cells Brodt, Matthew; Wycisk, Ryszard; Pintauro, Peter N. Journal of The Electrochemical Society, Vol. 160, Issue 8 https://doi.org/10.1149/2.008308jes	journal	January 2013
Nika : software for two-dimensional data reduction Ilavsky, Jan Journal of Applied Crystallography, Vol. 45, Issue 2 https://doi.org/10.1107/S0021889812004037	journal	March 2012
PEFC catalyst layers: Effect of support microstructure on both distributions of Pt and ionomer and cell performance and durability Uchida, Makoto Current Opinion in Electrochemistry, Vol. 21 https://doi.org/10.1016/j.coelec.2020.02.019	journal	June 2020
Catalyst-Layer Ionomer Imaging of Fuel Cells Guetaz, L.; Lopez-Haro, M.; Escribano, S. ECS Transactions, Vol. 69, Issue 17 https://doi.org/10.1149/06917.0455ecst	journal	September 2015
Comparative investigation into the performance and durability of long and short side chain ionomers in Polymer Electrolyte Membrane Fuel Cells Talukdar, Krishan; Gazdzicki, Pawel; Friedrich, K. Andreas Journal of Power Sources, Vol. 439 https://doi.org/10.1016/j.jpowsour.2019.227078	journal	November 2019
Recent advances in activity and durability enhancement of Pt/C catalytic cathode in PEMFC Yu, Xingwen; Ye, Siyu Journal of Power Sources, Vol. 172, Issue 1 https://doi.org/10.1016/j.jpowsour.2007.07.049	journal	October 2007
Humidity and Temperature Dependences of Oxygen Transport Resistance of Nafion Thin Film on Platinum Electrode Kudo, Kenji; Jinnouchi, Ryosuke; Morimoto, Yu Electrochimica Acta, Vol. 209 https://doi.org/10.1016/j.electacta.2016.04.023	journal	August 2016
Controlling Nafion Structure and Properties via Wetting Interactions Modestino, Miguel A.; Kusoglu, Ahmet; Hexemer, Alexander Macromolecules, Vol. 45, Issue 11, p. 4681-4688 https://doi.org/10.1021/ma300212f	journal	May 2012
Cathode Loading Impact on Voltage Cycling Induced PEMFC Degradation: A Voltage Loss Analysis Harzer, Gregor S.; Schwämmlein, Jan N.; Damjanović, Ana Marija Journal of The Electrochemical Society, Vol. 165, Issue 6 https://doi.org/10.1149/2.0161806jes	journal	January 2018
Effect of the Side-Chain Structure of Perfluoro-Sulfonic Acid Ionomers on the Oxygen Reduction Reaction on the Surface of Pt Kodama, Kensaku; Motobayashi, Kenta; Shinohara, Akihiro ACS Catalysis, Vol. 8, Issue 1 https://doi.org/10.1021/acscatal.7b03571	journal	December 2017
An in situ technique for analyzing ionomer coverage in catalyst layers Iden, Hiroshi; Ohma, Atsushi Journal of Electroanalytical Chemistry, Vol. 693 https://doi.org/10.1016/j.jelechem.2013.01.026	journal	March 2013
Study of the charge displacement at constant potential during CO adsorption on Pt(110) and Pt(111) electrodes in contact with a perchloric acid solution Clavilier, J.; Albalat, R.; Gomez, R. Journal of Electroanalytical Chemistry, Vol. 330, Issue 1-2 https://doi.org/10.1016/0022-0728(92)80326-Y	journal	July 1992
Effect of the catalytic ink preparation method on the performance of polymer electrolyte membrane fuel cells Shin, S. -J.; Lee, J. -K.; Ha, H. -Y. Journal of Power Sources, Vol. 106, Issue 1-2 https://doi.org/10.1016/S0378-7753(01)01045-X	journal	April 2002
Modifying the Electrocatalyst–Ionomer Interface via Sulfonated Poly(ionic liquid) Block Copolymers to Enable High-Performance Polymer Electrolyte Fuel Cells Li, Yawei; Van Cleve, Tim; Sun, Rui ACS Energy Letters, Vol. 5, Issue 6 https://doi.org/10.1021/acsenergylett.0c00532	journal	April 2020
Fuel-Cell Catalyst-Layer Resistance via Hydrogen Limiting-Current Measurements Schuler, Tobias; Chowdhury, Anamika; Freiberg, Anna T. Journal of The Electrochemical Society, Vol. 166, Issue 7 https://doi.org/10.1149/2.0031907jes	journal	January 2019
Agglomerates in Polymer Electrolyte Fuel Cell Electrodes: Part I. Structural Characterization Cetinbas, Firat C.; Ahluwalia, Rajesh K.; Kariuki, Nancy N. Journal of The Electrochemical Society, Vol. 165, Issue 13 https://doi.org/10.1149/2.0571813jes	journal	January 2018
On the Micro-, Meso-, and Macroporous Structures of Polymer Electrolyte Membrane Fuel Cell Catalyst Layers Soboleva, Tatyana; Zhao, Xinsheng; Malek, Kourosh ACS Applied Materials & Interfaces, Vol. 2, Issue 2 https://doi.org/10.1021/am900600y	journal	January 2010
Proton Conduction and Oxygen Reduction Kinetics in PEM Fuel Cell Cathodes: Effects of Ionomer-to-Carbon Ratio and Relative Humidity Liu, Yuxiu; Murphy, Michael W.; Baker, Daniel R. Journal of The Electrochemical Society, Vol. 156, Issue 8 https://doi.org/10.1149/1.3143965	journal	January 2009

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